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We introduce a hybrid technique that combines the robustness of frequency-resolved coherent anti-Stokes Raman scattering (CARS) with the advantages of time-resolved CARS spectroscopy. Instantaneous coherent broadband excitation of several characteristic molecular vibrations and the subsequent probing of these vibrations by an optimally shaped time-delayed(More)
We demonstrate broadband light generation by focusing two-color ultrashort laser pulses into a Raman-active crystal, lead tungstate (PbWO(4)). As many as 20 anti-Stokes and 2 Stokes fields are generated due to strong near-resonant excitation of a Raman transition. The generated spectrum extends from the infrared, through the visible region, to the(More)
We demonstrate broadband light generation in diamond pumped by two-color femtosecond laser pulses. We find that phase matching plays a critical role in the output angle and frequency of the generated sidebands. When a third femtosecond probe pulse is applied to the crystal in the boxed Coherent anti-Stokes Raman Scattering geometry, a two-dimensional array(More)
We develop a technique for optimizing the phase of broad spectrally-separated frequency sidebands-a "holey" spectrum. We use a source of multiple-order coherent Raman sidebands, obtained by crossing femtosecond pump and Stokes beams in synthetic single-crystal diamond. We combine the sidebands into a single beam and show the phase coherence among the(More)
We have generated multi-color optical vortices in a Raman-active crystal PbWO4 using two-color Fourier-transform limited femtosecond laser pulses. This setup overcomes some of the limitation of our previous research by allowing for the production of subcycle femtosecond optical vortices without the need for compensating for added chirp. In addition, the use(More)
Coherent Raman sidebands have the potential to serve as a source of single cycle pulses. We generate these sidebands by crossing two-color femtosecond laser pulses in a Raman-active crystal. We design a reflection scheme using spherical mirrors to combine coherent Raman sidebands. The sidebands and the driving pulses are refocused back to the Raman crystal(More)
We report pulse-shaper-assisted phase control of a broad spectrum, aiming to synthesize nonsinusoidal waveforms. We first generate multiple-order coherent Raman sidebands by focusing two laser beams into a piece of diamond. Then we combine five sidebands into a single beam by using a prism. Our setup allows for both coarse, manual phase adjustments and fine(More)
Experimental results from the generation of Raman sidebands using optical vortices are presented. By generating two sets of sidebands originating from different locations in a Raman-active crystal, one set containing optical orbital angular momentum and the other serving as a reference, Young's double slit experiment was simultaneously realized for each(More)
An octave-spanning coherent supercontinuum is generated by non-collinear Raman-assisted four-wave mixing in single-crystal diamond using 7.7 fs laser pulses that have been chirped to about 420 fs in duration. The use of ultrabroad bandwidth pulses as input results in substantial overlap of the generated spectrum of the anti-Stokes sidebands, creating a(More)
We study interference between a local oscillator and coherent anti-Stokes Raman scattering signal fields by controlling their relative phase and amplitude. This control allows direct observation of the real and imaginary components of the third-order nonlinear susceptibility (chi((3))) of the sample. In addition, we demonstrate that the heterodyne method(More)